析氧
催化作用
化学
电催化剂
纳米颗粒
电解质
电池(电)
化学工程
分解水
煅烧
制氢
纳米技术
无机化学
电极
物理化学
电化学
材料科学
热力学
有机化学
功率(物理)
物理
光催化
工程类
作者
Shadab Saifi,Gargi Dey,Renna Shakir,J. Karthikeyan,Ravi Kumar,D. Bhattacharyya,Amit Sinha,A. Aijaz
出处
期刊:Inorganic Chemistry
[American Chemical Society]
日期:2024-04-09
卷期号:63 (16): 7218-7232
被引量:1
标识
DOI:10.1021/acs.inorgchem.3c04443
摘要
Designing highly active and robust earth abundant trifunctional electrocatalysts for energy storage and conversion applications remain an enormous challenge. Herein, we report a trifunctional electrocatalyst (CrCo/CoN4@CNT-5), synthesized at low calcination temperature (550 °C), which consists of Co–N4 single atom and CrCo alloy nanoparticles and exhibits outstanding electrocatalytic performance for the hydrogen evolution reaction, oxygen evolution reaction, and oxygen reduction reaction. The catalyst is able to deliver a current density of 10 mA cm–2 in an alkaline electrolytic cell at a very low cell voltage of ∼1.60 V. When the catalyst is equipped in a liquid rechargeable Zn–air battery, it endowed a high open-circuit voltage with excellent cycling durability and outperformed the commercial Pt/C+IrO2 catalytic system. Furthermore, the Zn–air battery powered self-driven water splitting system is displayed using CrCo/CoN4@CNT-5 as sole trifunctional catalyst, delivering a high H2 evolution rate of 168 μmol h–1. Theoretical calculations reveal synergistic interaction between Co–N4 active sites and CrCo nanoparticles, favoring the Gibbs free energy for H2 evolution. The presence of Cr not only enhances the H2O adsorption and dissociation but also tunes the electronic property of CrCo nanoparticles to provide optimized hydrogen binding capacity to Co–N4 sites, thus giving rise to accelerated H2 evolution kinetics. This work highlights the importance of the presence of small quantity of Cr in enhancing the electrocatalytic activity as well as robustness of single-atom catalyst and suggests the design of the multifunctional robust electrocatalysts for long-term H2 evolution application.
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